Biaxially aligned YSZ thin films with strong [100] fiber texture were formed on a polycrystalline Ni-based alloy by off-normal ion-beam-assisted deposition. Growth structures were characterized by x-ray diffraction (XRD), transmission electron microscopy (TEM), atomic force microscopy (AFM), etc., and the alignment mechanism was discussed using a selective growth model. Peculiar structural evolution of the crystalline orientation was observed and its development was well described by an exponential equation. It was explained as a collaboration of an anisotropic growth condition and epitaxial crystallization. The [100] fiber texture was formed by columnar structures of diameter of 30 -100 nm, which were composed of 5-10 nm diameter crystallites. Very smooth surfaces were observed by AFM imaging with a roughness of 2-3 nm and a peculiar ripple structure. The origin of the azimuthal alignment was discussed with emphasis on the surface structure of YSZ films produced using ion-beam-assisted deposition (IBAD) and the etching rate measurements of (100) surfaces of YSZ single crystals.